Single‐Atom Fe‐Nx‐C as an Efficient Electrocatalyst for Zinc–Air Batteries

Highly efficient non‐noble metal electrocatalysts are vital for metal–air batteries and fuel cells. Herein, a noble‐metal–free single‐atom Fe‐N x‐C electrocatalyst is synthesized by incorporating Fe‐Phen complexes into the nanocages in situ during the growth of ZIF‐8, followed by pyrolysis at 900 °C under inert atmosphere. Fe‐Phen species provide both Fe2+ and the organic ligand (Phen) simultaneously, which play significant roles in preparing single‐atom catalysts. The obtained Fe‐Nx‐C exhibits a half‐wave potential of 0.91 V for the oxygen reduction reaction, higher than that of commercial Pt/C (0.82 V). As a cathode catalyst for primary zinc–air batteries (ZABs), the battery shows excellent electrochemical performances in terms of the high open‐circuit voltage (OCV) of 1.51 V and a high power density of 96.4 mW cm−2. The rechargeable ZAB with Fe‐Nx‐C catalyst and the alkaline electrolyte shows a remarkable cycling performance for 300 h with an initial round‐trip efficiency of 59.6%. Furthermore, the rechargeable all‐solid‐state ZABs with the Fe‐Nx‐C catalyst show high OCV of 1.49 V, long cycle life for 120 h, and foldability. The single‐atom Fe‐Nx‐C electrocatalyst may function as a promising catalyst for various metal–air batteries and fuel cells. A single‐atom iron catalyst (Fe‐Nx‐C) is prepared by pyrolysis of Fe‐Phen@ZIF‐8. Fe‐Nx‐C exhibits a higher half‐wave potential than that of Pt/C. As a cathode catalyst for the primary and the rechargeable all‐solid‐state zinc–air batteries, Fe‐Nx‐C shows excellent electrochemical performances in terms of high open‐circuit voltage, high power density, remarkable cyclability, and the foldable property.